PNNL

Abstract

This review offers a succinct overview of the development of a vacuum compatible microfluidic reactor, system for analysis at the liquid vacuum interface (SALVI), and its diverse applications in in situ, in vivo, and in operando imaging of liquid surfaces as well as the air-liquid (a-l), liquid-liquid (l-l), and solid-liquid (s-l) interfaces in the past decade. SALVI is one of the first microfluidics-based reactors that has enabled direct analysis of volatile liquids in vacuum surface tools such as scanning electron microscopy (SEM) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Its integration into ambient and vacuum spectroscopy and microscopy is illustrated. Several applications are highlighted including 1) imaging nano particles in liquid using in situ SEM; 2) mapping the evolving l-l interface using in situ x-ray absorption spectroscopy (XAS) and ToF-SIMS; 3) following complex air-liquid interfacial oxidation reaction products using in situ ToF-SIMS; 4) capturing biological interfaces of cells and microbes via in vivo multimodal and correlative imaging; and 5) monitoring the dynamic solid electrode and liquid electrolyte interface using in operando molecular imaging . Finally, outlook and recommendations are presented. Besides showing the holistic information volume obtained by real-time multiplexed imaging, this review intends to convey the importance of tool development in revolutionizing surface and interface analysis using vacuum platforms previously limited to solid surfaces. Microfluidics is manifested to be not limited to ambient conditions in many examples in this review. Moreover, fundamental interfacial phenomena underpinning mass and charge transfer can now be pursued in real time via innovated chemical imaging and spectroscopy.